WO2012117661A1 - Pile à combustible - Google Patents

Pile à combustible Download PDF

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Publication number
WO2012117661A1
WO2012117661A1 PCT/JP2012/000502 JP2012000502W WO2012117661A1 WO 2012117661 A1 WO2012117661 A1 WO 2012117661A1 JP 2012000502 W JP2012000502 W JP 2012000502W WO 2012117661 A1 WO2012117661 A1 WO 2012117661A1
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WO
WIPO (PCT)
Prior art keywords
catalyst layer
fuel cell
electrolyte membrane
reinforcing layer
layer
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Application number
PCT/JP2012/000502
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English (en)
Japanese (ja)
Inventor
匡志 藤澤
礒野　隆博
Original Assignee
三洋電機株式会社
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Filing date
Publication date
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Publication of WO2012117661A1 publication Critical patent/WO2012117661A1/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8663—Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M2008/1095—Fuel cells with polymeric electrolytes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the present invention relates to a fuel cell, and more particularly to a fuel cell in which a plurality of membrane electrode assemblies are arranged in a plane.
  • Fuel cells are devices that generate electrical energy from hydrogen and oxygen, and can achieve high power generation efficiency.
  • the main features of the fuel cell are direct power generation that does not go through the process of thermal energy and kinetic energy as in the conventional power generation method, so that high power generation efficiency can be expected even on a small scale, and there is little emission of nitrogen compounds, Noise and vibration are also small, so the environmental performance is good.
  • the fuel cell can effectively use the chemical energy of fuel and has environmentally friendly characteristics, so it is expected as an energy supply system for the 21st century, from space use to automobiles and portable devices. It is attracting attention as a promising new power generation system that can be used for various applications from large-scale power generation to small-scale power generation, and technological development is in full swing toward practical application.
  • solid polymer fuel cells are characterized by low operating temperature and high output density compared to other types of fuel cells.
  • mobile devices for example, mobile phones, notebook personal computers, Use in power sources such as PDAs, MP3 players, digital cameras or electronic dictionaries, electronic books
  • a polymer electrolyte fuel cell for portable equipment a planar array type fuel cell in which a plurality of membrane electrode assemblies (single cells) are arranged in a planar shape is known (see Patent Document 1).
  • Each membrane electrode assembly has a structure in which an anode catalyst layer is provided on one surface of an electrolyte membrane containing a proton exchanger, and a cathode catalyst layer is provided on the other surface.
  • a power generation reaction is performed in a state where the electrolyte membrane and the catalyst layer are humidified in order to promote proton exchange in the electrolyte membrane. Therefore, when the fuel cell is used, the electrolyte membrane and the catalyst layer are repeatedly changed between a wet state and a dry state.
  • the electrolyte membrane is more likely to swell than the catalyst layer. For this reason, when the fuel cell is used for a long period of time and the wet state of the electrolyte membrane and the catalyst layer is repeated, both of them repeatedly swell, and as a result, there is a possibility that cracks occur in the catalyst layer. When a crack occurs in the catalyst layer, the electrical conductivity is lowered or the contact resistance between the electrolyte membrane and the catalyst layer is increased in the crack generation portion. As a result, the internal resistance of the fuel cell increases and the power generation performance of the fuel cell decreases.
  • the present invention has been made in view of these problems, and an object of the present invention is to provide a technique for suppressing the generation of cracks in the catalyst layer and avoiding a decrease in power generation performance of the fuel cell.
  • the fuel cell includes an electrolyte membrane including an ion exchanger, an anode catalyst layer provided on one surface of the electrolyte membrane, a membrane electrode assembly having a cathode catalyst layer provided on the other surface of the electrolyte membrane, and an anode A reinforcing layer embedded in at least one of the catalyst layer and the cathode catalyst layer and having an area projected onto a plane parallel to the main surface of the electrolyte membrane is smaller than the catalyst layer and is less likely to swell than the electrolyte membrane. It is characterized by.
  • FIG. 1 is an exploded perspective view showing a schematic configuration of a fuel cell according to Embodiment 1.
  • FIG. FIG. 2A is a cross-sectional view taken along the line AA in FIG.
  • FIG. 2B is a cross-sectional view along the line BB in FIG.
  • FIG. 3A is an enlarged view of a region surrounded by a broken line in FIG.
  • FIG. 3B is a schematic view showing a modification of the structure of the reinforcing layer.
  • 4A to 4C are process cross-sectional views illustrating the method of manufacturing the fuel cell according to the first embodiment.
  • 5A to 5C are process cross-sectional views illustrating the method of manufacturing the fuel cell according to the first embodiment.
  • FIG. 6A and 6B are process cross-sectional views illustrating the method for manufacturing the fuel cell according to the first embodiment.
  • FIG. 7A is a plan view showing a schematic structure of a fuel cell according to Embodiment 2.
  • FIG. 7B is a cross-sectional view taken along the line DD in FIG. 6 is a cross-sectional view showing a schematic configuration of a membrane electrode assembly provided in a fuel cell according to Embodiment 3.
  • FIG. It is sectional drawing which shows schematic structure of the membrane electrode assembly with which the fuel cell which concerns on Embodiment 4 is provided.
  • FIG. 10A is a plan view showing a schematic configuration of a membrane electrode assembly provided in the fuel cell according to Embodiment 5.
  • FIG. 10B is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 5-1.
  • FIG. 10C is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 5-2.
  • FIG. 10D is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 5-3.
  • FIG. 11A is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 5-4.
  • FIG. 11B is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 5-5.
  • FIG. 12A is a plan view showing a schematic configuration of a membrane electrode assembly provided in the fuel cell according to Embodiment 6.
  • FIG. 12B is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-1.
  • FIG. 12C is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-2.
  • FIG. 12D is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-3.
  • FIG. 13A is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-4.
  • FIG. 13B is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-5.
  • FIG. 13C is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-6.
  • FIG. 14A is a plan view showing a schematic configuration of a membrane electrode assembly provided in the fuel cell according to Embodiment 7.
  • FIG. 14B is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 7-1.
  • FIG. 1 is an exploded perspective view showing a schematic configuration of a fuel cell according to Embodiment 1.
  • FIG. FIG. 2A is a cross-sectional view taken along the line AA in FIG.
  • FIG. 2B is a cross-sectional view along the line BB in FIG.
  • FIG. 3A is an enlarged view of a region surrounded by a broken line in FIG.
  • FIG. 3B is a schematic view showing a modification of the structure of the reinforcing layer.
  • each of a plurality of fiber materials 132 which will be described later, is represented by a small circle for convenience, but the plurality of fiber materials 132 are arranged in the same direction in the reinforcing layer 130. Does not extend along.
  • the fuel cell 10 includes a plurality of membrane electrode assemblies (MEAs) 100, a reinforcing layer 130, A cathode housing 50 and an anode housing 52 are provided.
  • MEAs membrane electrode assemblies
  • the plurality of membrane electrode assemblies 100 are disposed in the openings 112 provided in the base 110 and are arranged in a plane.
  • the base material 110 is formed of an insulating material such as polyester.
  • the thickness of the base material 110 is, for example, about 30 ⁇ m.
  • the opening 112, that is, the length of the membrane electrode assembly 100 For example, the thickness is about 2000 ⁇ m.
  • Each membrane electrode assembly 100 includes an electrolyte membrane 102, an anode catalyst layer 104 provided on one surface of the electrolyte membrane 102, and a cathode catalyst layer 106 provided on the other surface of the electrolyte membrane 102.
  • a cell is configured by sandwiching the electrolyte membrane 102 between the pair of anode catalyst layers 104 and the cathode catalyst layer 106.
  • Hydrogen is supplied to the anode catalyst layer 104 as a fuel gas. In this embodiment, hydrogen is used as the fuel gas, but other suitable fuels such as methanol, formic acid, butane, or other hydrogen carriers can be used.
  • Air is supplied to the cathode catalyst layer 106 as an oxidant.
  • Each cell, that is, each membrane electrode assembly 100 generates power by an electrochemical reaction between hydrogen and oxygen in the air.
  • the electrolyte membrane 102 preferably exhibits good ionic conductivity in a wet state, and functions as an ion exchange membrane that moves protons between the anode catalyst layer 104 and the cathode catalyst layer 106.
  • the electrolyte membrane 122 is formed of a solid polymer material (ion exchanger) such as a fluorine-containing polymer or a non-fluorine polymer, and includes, for example, a sulfonic acid type perfluorocarbon polymer, a polysulfone resin, a phosphonic acid group, or a carboxylic acid group.
  • a perfluorocarbon polymer having the same can be used.
  • Examples of the sulfonic acid type perfluorocarbon polymer include Nafion (registered trademark) membrane (manufactured by DuPont).
  • Examples of non-fluorine polymers include sulfonated aromatic polyetheretherketone and polysulfone.
  • the thickness of the electrolyte membrane 122 is, for example, about 30 ⁇ m.
  • the anode catalyst layer 104 and the cathode catalyst layer 106 have ion exchangers and catalyst particles, and possibly carbon particles.
  • the ion exchangers included in the anode catalyst layer 104 and the cathode catalyst layer 106 may be used to improve the adhesion between the catalyst particles and the electrolyte membrane 102, and may have a role of transmitting protons between the two. Good.
  • This ion exchanger can be formed from the same polymer material as the electrolyte membrane 102.
  • catalyst metals include Sc, Y, Ti, Zr, V, Nb, Fe, Co, Ni, Ru, Rh, Pd, Pt, Os, Ir, alloys selected from lanthanoid series elements and actinoid series elements, A simple substance is mentioned. When the catalyst is supported, furnace black, acetylene black, ketjen black, carbon nanotubes or the like may be used as the carbon particles.
  • Each of the anode catalyst layer 104 and the cathode catalyst layer 106 has a thickness of about 50 ⁇ m, for example.
  • the reinforcing layer 130 is a substantially plate-like member that is less likely to swell than the electrolyte membrane 102 and is embedded in the cathode catalyst layer 106.
  • the characteristic of the reinforcing layer 130 that it is less likely to swell than the electrolyte membrane 102 is that the reinforcing layer 130 includes a fiber material 132 that is less likely to swell than the electrolyte membrane 102 as shown in FIG. It is realized with. Examples of such a fiber material 132 include carbon nanofibers.
  • the thickness, width, and length of the reinforcing layer 130 are about 20 ⁇ m, about 200 ⁇ m, and about 2000 ⁇ m, respectively.
  • the thickness and width of the reinforcing layer 130 are the length in the vertical direction and the length in the horizontal direction in the cross section perpendicular to the extending direction of the reinforcing layer 130 (the cross section shown in FIG. 2B). .
  • the catalyst particles of the cathode catalyst layer 106 that are arranged above the reinforcing layer 130 and are not in direct contact with the electrolyte membrane 102 move according to the swelling of the electrolyte membrane 102. There is nothing to do. Alternatively, the amount of movement is smaller than that of the catalyst particles of the cathode catalyst layer 106 that is in direct contact with the electrolyte membrane 102. Therefore, by embedding the reinforcing layer 130 in the cathode catalyst layer 106, it is possible to suppress the occurrence of cracks in the cathode catalyst layer 106.
  • the surface of the reinforcing layer 130 is uneven by the fiber material located in the vicinity of the surface of the reinforcing layer 130. Thereby, the adhesion between the reinforcing layer 130 and the cathode catalyst layer 106 is enhanced. As a result, the expansion of the cathode catalyst layer 106 accompanying the swelling of the electrolyte membrane 102 can be further suppressed.
  • the fiber material 132 in contact with the cathode catalyst layer 106 is covered with an ion exchanger 133 that is the same material as the ion exchanger included in the electrolyte membrane 102. Since the ion exchanger 133 is also included in the cathode catalyst layer 106, the adhesion between the reinforcing layer 130 and the cathode catalyst layer 106 can be improved. Thereby, since the movement of the catalyst particles of the cathode catalyst layer 106 accompanying the swelling of the electrolyte membrane 102 can be further suppressed, the occurrence of cracks in the cathode catalyst layer 106 can be further suppressed.
  • the reinforcing layer 130 has conductivity. Since the carbon nanofibers described above have good electrical conductivity, they can be suitably employed as the fiber material 132 that makes the reinforcing layer 130 conductive. Since the reinforcing layer 130 has conductivity, it is possible to avoid a decrease in conductivity in the cathode catalyst layer 106 due to the provision of the reinforcing layer 130.
  • the reinforcing layer 130 is provided in contact with the electrolyte membrane 102.
  • the swelling of the electrolyte membrane 102 in the portion in contact with the reinforcing layer 130 can be suppressed. Therefore, the occurrence of cracks in the cathode catalyst layer 106 can be suppressed.
  • the adhesion between the reinforcing layer 130 and the electrolyte membrane 102 is enhanced by the unevenness formed on the surface of the reinforcing layer 130, the occurrence of cracks in the cathode catalyst layer 106 can be further suppressed. Note that the occurrence of cracks in the cathode catalyst layer 106 can be suppressed only by suppressing the swelling of the electrolyte membrane 102 by the adhesion between the reinforcing layer 130 and the electrolyte membrane 102.
  • the maximum length of the fiber material 132 included in the reinforcing layer 130 is set to be less than the thickness of the electrolyte membrane 102.
  • the reinforcing layer 130 is formed by spraying a fiber material 132 onto the surface of the electrolyte membrane 102. Therefore, by setting the maximum length of the fiber material 132 to be less than the thickness of the electrolyte membrane 102, the fiber material 132 sprayed on the surface of the electrolyte membrane 102 can be prevented from penetrating the electrolyte membrane 102.
  • the reinforcing layer 130 may be formed of an integral flat plate member.
  • a Teflon (registered trademark) plate, a carbon plate, or the like can be adopted.
  • the amount of biting into the surface of the electrolyte membrane 102 of the material which comprises the reinforcement layer 130 can be reduced. Therefore, the above-described short circuit and cross leak can be prevented more reliably.
  • the adhesion between the electrolyte membrane 102 and the reinforcing layer 130 is lower than when the surface is formed of the fiber material 132. Therefore, the function of suppressing the swelling of the electrolyte membrane 102 by the reinforcing layer 130 is reduced. In addition, the adhesion between the reinforcing layer 130 and the cathode catalyst layer 106 also decreases. As a result, the cathode catalyst layer 106 located above the reinforcing layer 130 is easily pulled by the swelling of the electrolyte membrane 102. Therefore, as shown in FIG.
  • the reinforcing layer 130 is formed by a flat plate member 134 in contact with the surface of the electrolyte membrane 102 and a fiber material 132 deposited on the surface of the flat plate member 134. The surface is brought into contact with the electrolyte membrane 102. As a result, it is possible to avoid the occurrence of cracks in the cathode catalyst layer 106 due to swelling of the electrolyte membrane 102 while preventing the occurrence of the short circuit and the cross leak described above.
  • the area of the reinforcing layer 130 projected onto a plane parallel to the main surface of the electrolyte membrane 102 is smaller than the area of the cathode catalyst layer 106. That is, the reinforcing layer 130 has a smaller area than the cathode catalyst layer 106 in plan view. Thereby, the area
  • the reinforcing layer 130 preferably has an area occupied by the cathode catalyst layer 106 provided with the reinforcing layer 130 in a plan view of 10% or less.
  • the reinforcing layer 130 may be embedded in the anode catalyst layer 104.
  • An interconnector 140 extends at the boundary between adjacent membrane electrode assemblies 100.
  • the substrate 110 is provided with a slit 114 between adjacent openings 112, and the interconnector 140 is provided so as to pass through the slit 114.
  • One end of the interconnector 140 extends toward the anode catalyst layer 104 of the one membrane electrode assembly 100, and the other end of the interconnector 140 is the cathode catalyst layer of the other membrane electrode assembly 100. It extends towards 106.
  • the interconnector 140 is made of a conductive material such as carbon.
  • One end portion of the interconnector 140 extending toward the anode catalyst layer 104 is in contact with the side surface of the anode catalyst layer 104.
  • the other end of the anode catalyst layer 104 extending toward the cathode catalyst layer 106 is in contact with the side surface of the cathode catalyst layer 106. Accordingly, one anode catalyst layer 104 and the other cathode catalyst layer 106 of the adjacent membrane electrode assembly 100 are electrically connected via the interconnector 140, and the adjacent membrane electrode assemblies 100 are connected in series. ing.
  • the anode catalyst layers 104 and the cathode catalyst layers 106 of the adjacent membrane electrode assemblies 100 are insulated from each other.
  • the width of the interconnector 140 in plan view that is, the width from the end in contact with the anode catalyst layer 104 to the end in contact with the cathode catalyst layer 106 is, for example, about 600 ⁇ m.
  • a current collector 150 is connected to the anode catalyst layer 104 ′ that is one end of the series connection of the plurality of membrane electrode assemblies 100 and the cathode catalyst layer 106 ′ that is the other end.
  • the reinforcing layer 130 extends in a direction intersecting with the interconnector 140.
  • the reinforcing layer 130 extends substantially perpendicular to the interconnector 140.
  • the reinforcing layer 130 extends from the end of the cathode catalyst layer 106 on the side in contact with the interconnector 140 to the other end facing the end. Therefore, it is possible to suppress the occurrence of cracks extending in a direction substantially perpendicular to the conductive direction over the entire conductive direction in the cathode catalyst layer 106.
  • one end of the reinforcing layer 130 is in contact with the interconnector 140.
  • the cathode catalyst layer 106 is in contact with the interconnector 140 at a portion disposed above the reinforcing layer 130.
  • a decrease in conductivity in the cathode catalyst layer 106 can be further suppressed.
  • a protruding portion 130 a extending on the upper surface of the interconnector 140 is provided at one end of the reinforcing layer 130. A part of the upper surface of the interconnector 140 is covered with the protruding portion 130a.
  • the cathode catalyst layer 106 ′ that is the terminal end of the series connection of the plurality of membrane electrode assemblies 100 is in contact with the current collector 150.
  • the cathode catalyst layer 106 is in contact with the current collector 150 at a portion disposed above the reinforcing layer 130.
  • a protrusion 130 a is provided at one end of the reinforcing layer 130, and a part of the upper surface of the current collector 150 is covered with the protrusion 130 a.
  • the cathode housing 50 is a plate-like member facing the cathode catalyst layer 106.
  • the cathode housing 50 is provided with a plurality of air intakes 51 for taking in air from the outside.
  • An air chamber 60 through which air flows is formed between the cathode housing 50 and the cathode catalyst layer 106.
  • the anode housing 52 is a plate-like member facing the anode catalyst layer 104.
  • a fuel gas chamber 62 for storing fuel is formed between the anode housing 52 and the anode catalyst layer 104.
  • fuel supply port (not shown) in the anode housing 52, fuel can be appropriately replenished from a fuel cartridge or the like.
  • Examples of materials used for the cathode housing 50 and the anode housing 52 include general plastic resins such as phenol resin, vinyl resin, polyethylene resin, polypropylene resin, polystyrene resin, urea resin, and fluorine resin.
  • the gasket 56 is provided between the outer periphery of the substrate 110 and the anode housing 52.
  • the gasket 56 improves the sealing performance of the fuel gas chamber 62 and suppresses fuel leakage.
  • the gasket 57 is provided between the outer periphery of the base 110 and the cathode housing 50.
  • a base material 110 is prepared.
  • a plurality of openings 112 and slits 114 are formed in the substrate 110.
  • the slit 114 is formed between adjacent openings 112.
  • the width of the slit 114 is about 200 ⁇ m, and the distance between the opening 112 and the slit 114 is about 200 ⁇ m.
  • a method of forming the opening 112 and the slit 114 for example, laser processing using an infrared laser, visible light laser, ultraviolet laser, or the like, or a punching method using a mold can be employed.
  • the electrolyte membrane 102 is formed in the opening 112 provided in the substrate 110.
  • the electrolyte membrane 102 can be formed by filling the opening 112 with a Nafion solution and then evaporating the solvent.
  • the electrolyte membrane 102 that has been molded in advance to the size of the opening 112 may be fitted into the opening 112.
  • the Nafion solution is poured into the interface between the substrate 110 and the electrolyte membrane 102 after the electrolyte membrane 102 is fitted into the opening 112. According to this, since the Nafion solution functions as an adhesive, the adhesion between the substrate 110 and the electrolyte membrane 102 can be improved.
  • the interconnector 140 is inserted into the slit 114 provided in the substrate 110.
  • the interconnector 140 inserted through the slit 114 has one end bent to the one electrolyte membrane 102 side and the other end bent to the other electrolyte membrane 102 side.
  • a current collector 150 is provided on one main surface side of the substrate 110 and on one end portion in the longitudinal direction, and on the other main surface side of the substrate 110 and on the other end portion in the longitudinal direction. Provided.
  • a mask 200 having an opening 202 in a region where the reinforcing layer 130 is to be formed is laminated on one main surface side of the substrate 110.
  • the mask 200 is provided with a plurality of openings 202 corresponding to the formation region of the electrolyte membrane 102.
  • the opening 202 extends substantially perpendicular to the interconnector 140 and the current collector 150.
  • One end of the opening 202 extends to a position overlapping the end of the electrolyte membrane 102, and the other end of the opening 202 extends to a position where a part of the interconnector 140 or current collector 150 is exposed. Yes.
  • the fiber material 132 (see FIG. 3A, etc.) constituting the reinforcing layer 130 is spray-applied into the opening 202 of the mask 200, so that the protruding portion 130a is formed.
  • the reinforcing layer 130 is formed.
  • the mask 200 is peeled off.
  • a catalyst layer 206 is formed along the longitudinal direction of the substrate 110 so as to straddle the plurality of electrolyte membranes 102.
  • various materials constituting the cathode catalyst layer 106 are sufficiently stirred to prepare a catalyst slurry, and the catalyst layer 206 is formed by spray coating the catalyst slurry.
  • the catalyst layer 204 is formed along the longitudinal direction of the substrate 110 so as to straddle the plurality of electrolyte membranes 102 on the other main surface side of the substrate 110.
  • the catalyst layer 204 is formed by spray-coating a catalyst slurry prepared by stirring various materials constituting the anode catalyst layer 104.
  • a catalyst layer located in a predetermined region of the catalyst layer 206 provided on one main surface side of the substrate 110, that is, a region sandwiched between adjacent electrolyte membranes 102. 206 is partially removed using a laser such as an excimer laser.
  • the cathode catalyst layer 106 is formed on each electrolyte membrane 102 by dividing the catalyst layer 206. Note that a part of the catalyst layer 206 located on the interconnector 140 and the catalyst layer 206 located on the current collector 150 are left without being removed by the laser.
  • a predetermined region of the catalyst layer 204 provided on the other main surface side of the substrate 110, that is, the catalyst layer 204 located in a region sandwiched between adjacent electrolyte membranes 102 is partially formed using a laser such as an excimer laser. To remove. By dividing the catalyst layer 204, the anode catalyst layer 104 located on each electrolyte membrane 102 is formed.
  • the laser output only needs to be sufficient to completely remove the catalyst layer in the laser irradiation portion, and may be adjusted as appropriate according to the material and thickness of the catalyst layer.
  • a cathode housing 50 is provided on one main surface side of the base material 110 via a gasket 57, and an anode housing is provided on the other main surface side of the base material 110 via a gasket 56.
  • the fuel cell 10 is formed.
  • the fuel cell 10 includes the reinforcing layer 130 embedded in the catalyst layer and having a smaller area than the catalyst layer in plan view and less likely to swell than the electrolyte membrane 102. Thereby, it is possible to suppress the occurrence of cracks due to swelling of the electrolyte membrane 102 in the catalyst layer in which the reinforcing layer 130 is embedded. As a result, a decrease in power generation performance of the fuel cell 10 can be avoided, and the life of the fuel cell 10 can be extended.
  • Embodiment 2 In the fuel cell 10 according to Embodiment 2, a plurality of reinforcing layers 130 are provided in the same catalyst layer.
  • the structure other than the reinforcing layer 130 of the fuel cell 10 is basically the same as that of the first embodiment.
  • the same components as those in the first embodiment are denoted by the same reference numerals, and the description thereof is omitted as appropriate.
  • FIG. 7A is a plan view showing a schematic structure of the fuel cell according to the second embodiment.
  • FIG. 7B is a cross-sectional view taken along the line DD in FIG.
  • the cathode catalyst layer 106 is represented by a broken line, and the cathode catalyst layer 106 is seen through.
  • a plurality of reinforcing layers 130 are provided on the cathode catalyst layer 106, two in this case.
  • the plurality of reinforcing layers 130 are arranged to extend in parallel with each other with a predetermined interval.
  • the area occupied by the reinforcing layer 130 with respect to the cathode catalyst layer 106 in plan view is set to be substantially equal to the configuration of the first embodiment in which one reinforcing layer 130 is provided. That is, also in this embodiment, the total occupied area of the reinforcing layer 130 with respect to the cathode catalyst layer 106 in a plan view is 10% or less. Accordingly, it is possible to avoid a decrease in the area where the electrolyte membrane 102 and the cathode catalyst layer 106 are in direct contact with each other by increasing the number of the reinforcing layers 130.
  • the conductivity of the cathode catalyst layer 106 can be increased.
  • the two reinforcing layers 130 are provided on the cathode catalyst layer 106.
  • the number of the reinforcing layers 130 is not particularly limited as long as the effect of suppressing the occurrence of cracks is obtained.
  • the plurality of reinforcing layers 130 may be provided on the anode catalyst layer 104. That is, if the plurality of reinforcing layers 130 are provided in at least one of the anode catalyst layer 104 and the cathode catalyst layer 106, the above-described catalyst layer on the side where the plurality of reinforcing layers 130 are embedded is described above. An effect can be obtained.
  • a plurality of reinforcing layers 130 are provided in the same catalyst layer. Further, by providing a plurality of reinforcing layers 130, an increase in the total occupied area of the reinforcing layers 130 with respect to the catalyst layer in a plan view is suppressed. As a result, it is possible to more reliably prevent the occurrence of cracks that run parallel to the direction in which the interconnector 140 extends, and to avoid a reduction in the area where the electrolyte membrane 102 and the cathode catalyst layer 106 are in direct contact.
  • the cross-sectional shape of the reinforcing layer 130 is different from that of the first embodiment.
  • this embodiment will be described.
  • the structure other than the reinforcing layer 130 of the fuel cell 10 is basically the same as that of the first embodiment.
  • the same components as those in the first embodiment are denoted by the same reference numerals, and the description thereof is omitted as appropriate.
  • FIG. 8 is a cross-sectional view showing a schematic configuration of a membrane electrode assembly provided in the fuel cell according to Embodiment 3. 8 is a cross-sectional view perpendicular to the extending direction of the reinforcing layer 130, and corresponds to a cross-sectional view along the line BB in FIG.
  • the reinforcing layer 130 has a contact area with the portion of the cathode catalyst layer 106 disposed above the reinforcing layer 130 in contact with the electrolyte membrane 102. It is formed so as to be larger than the area. That is, when viewed in a cross section perpendicular to the extending direction of the reinforcing layer 130, the length D1 of the contact portion with the cathode catalyst layer 106 disposed above the reinforcing layer 130 and the contact portion with the electrolyte membrane 102 are as follows. The length D2 satisfies the relationship of D1 ⁇ D2.
  • the contact area between the reinforcing layer 130 and the cathode catalyst layer 106 can be increased, and the adhesion between them can be improved.
  • the contact area between the reinforcing layer 130 and the electrolyte membrane 102 is reduced, in other words, the contact area between the electrolyte membrane 102 and the cathode catalyst layer 106 is increased, and the membrane obtained by providing the reinforcing layer 130. A decrease in power generation performance of the electrode assembly 100 can be suppressed.
  • the anode catalyst layer 104 and the cathode catalyst layer 106 are provided with the reinforcing layer 130, and the reinforcing layer 130 provided on the anode catalyst layer 104 and the cathode catalyst layer 106 are provided.
  • the positional relationship with the reinforcing layer 130 is determined.
  • this embodiment will be described.
  • the structure other than the reinforcing layer 130 of the fuel cell 10 is basically the same as that of the first embodiment.
  • the same components as those in the first embodiment are denoted by the same reference numerals, and the description thereof is omitted as appropriate.
  • FIG. 9 is a cross-sectional view showing a schematic configuration of a membrane electrode assembly provided in the fuel cell according to Embodiment 4.
  • 9 is a cross-sectional view perpendicular to the extending direction of the reinforcing layer 130, and corresponds to a cross-sectional view along the line BB in FIG.
  • the reinforcing layer 130 is embedded in the anode catalyst layer 104 and the cathode catalyst layer 106.
  • the reinforcing layer 130 embedded in the anode catalyst layer 104 and the reinforcing layer 130 embedded in the cathode catalyst layer 106 are projected onto a plane parallel to the main surface of the electrolyte membrane 102 (arrows in FIG. 9). Overlapping (when viewed from the Z direction). That is, the reinforcing layers 130 provided on both catalyst layers are provided at positions facing each other with the electrolyte membrane 102 interposed therebetween.
  • the efficiency of the power generation reaction tends to be lower than that in the region where the reinforcing layer 130 is not provided. Therefore, when the reinforcing layer 130 is provided on both the anode catalyst layer 104 and the cathode catalyst layer 106, the reinforcing layers 130 provided on both catalyst layers are arranged so as to overlap in plan view. Thereby, the increase in the area
  • the reinforcing layer 130 embedded in the anode catalyst layer 104 and the reinforcing layer 130 embedded in the cathode catalyst layer 106 can obtain the above-described effects to some extent as long as at least a part thereof overlaps in plan view. .
  • the fuel cell 10 according to the fifth embodiment is different from the first embodiment in the shape of the reinforcing layer 130 when viewed in plan.
  • this embodiment will be described.
  • the structure other than the reinforcing layer 130 of the fuel cell 10 is basically the same as that of the first embodiment.
  • the same components as those in the first embodiment are denoted by the same reference numerals, and the description thereof is omitted as appropriate.
  • FIG. 10A is a plan view showing a schematic configuration of a membrane electrode assembly provided in the fuel cell according to Embodiment 5.
  • FIG. 10B is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 5-1.
  • FIG. 10C is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 5-2.
  • FIG. 10D is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 5-3.
  • FIG. 11A is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 5-4.
  • FIG. 11B is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 5-5.
  • the reinforcing layer 130 of the present embodiment has a shape that gradually expands as it approaches the interconnector 140 in plan view, that is, the extension direction of the interconnector 140 (interconnector as it approaches the interconnector 140).
  • the connector 140 and the cathode catalyst layer 106 have a shape in which the length (in the direction in which the interface extends) gradually increases.
  • the reinforcing layer 130 of the present embodiment has one side 136 positioned on the interconnector 140 side, and a vertex 138 facing the one side 136 at the end of the electrolyte membrane 102 opposite to the interconnector 140. It is a substantially triangular shape.
  • the length of one side 136 is longer than the width of the reinforcing layer 130 of the first embodiment.
  • the reinforcing layer 130 extends over the entire region in the extending direction of the interconnector 140.
  • the length of one side 136 and the distance from the apex 138 to one side 136 are both about 2000 ⁇ m, for example.
  • the reinforcing layer 130 has a shape that expands as the interconnector 140 is approached. Therefore, the extension range of the reinforcing layer 130 in the vicinity of the interconnector 140 can be widened as compared with the first embodiment. For example, when the area of the reinforcing layer 130 is the same in the first embodiment and the present embodiment, the extending range of the reinforcing layer 130 in the vicinity of the interconnector 140 is wider in the present embodiment than in the first embodiment.
  • Examples of the reinforcing layer 130 of the present embodiment include the following modified examples 5-1 to 5-5.
  • the vertex 138 of the reinforcing layer 130 is located closer to the interconnector 140 than in the fifth embodiment. That is, the reinforcing layer 130 of the modified example 5-1 has a triangular height smaller than that of the reinforcing layer 130 of the fifth embodiment when the one side 136 is the base.
  • the occurrence of cracks in the vicinity of the interconnector 140 can be suppressed to the same extent as in the fifth embodiment, and the contact area between the electrolyte membrane 102 and the cathode catalyst layer 106 can be increased as compared with the fifth embodiment.
  • a decrease in proton conductivity from the electrolyte membrane 102 to the cathode catalyst layer 106 can be suppressed.
  • the distance from the vertex 138 to one side 136 is, for example, about 1000 ⁇ m.
  • the reinforcing layer 130 of the modification 5-2 has a side 136 shorter than the side 136 of the reinforcing layer 130 of the fifth embodiment.
  • the reinforcing layer 130 of the modification 5-2 has a side 136 shorter than the side 136 of the reinforcing layer 130 of the fifth embodiment.
  • the reinforcing layer 130 of the modified example 5-1 can more reliably suppress the occurrence of cracks in the vicinity of the interconnector 140 than the modified example 5-2.
  • the length of one side 136 is, for example, about 1000 ⁇ m.
  • a plurality of reinforcing layers 130 may be arranged in the extending direction of the interconnector 140.
  • the reinforcing layer 130 of the modified example 5-3 has a shape in which the modified example 5-1 and the modified example 5-2 are combined, and the vertex 138 has an interface compared to the fifth embodiment. It is located from the connector 140 and the length of one side 136 is shorter than that of the fifth embodiment. As a result, it is possible to more reliably suppress the occurrence of cracks in the vicinity of the interconnector 140 as compared with the first embodiment, and as compared with the fifth embodiment, the modified example 5-1, and the modified example 5-2.
  • the contact area between the electrolyte membrane 102 and the cathode catalyst layer 106 can be increased to suppress a decrease in proton conductivity.
  • the length of one side 136 and the distance from the vertex 138 to one side 136 are both about 1000 ⁇ m, for example.
  • Modifications 5-4, 5-5) As shown in FIG. 11A, the reinforcing layer 130 of Modification 5-4 is different from Embodiment 5 in that it has a substantially semicircular shape. Further, as shown in FIG. 11B, the reinforcing layer 130 of the modified example 5-5 differs from the fifth embodiment in that it has a substantially trapezoidal shape. Even with these reinforcing layers 130, the occurrence of cracks in the vicinity of the interconnector 140 can be more reliably suppressed as compared to the first embodiment. Note that the reinforcement layer 130 of the modification 5-4 and the reinforcement layer 130 of the modification 5-5 can be modified in the same manner as the modifications 5-1 to 5-3 for the fifth embodiment.
  • the fuel cell 10 according to the sixth embodiment is different from the first embodiment in the shape of the reinforcing layer 130 when viewed in plan.
  • this embodiment will be described.
  • the structure other than the reinforcing layer 130 of the fuel cell 10 is basically the same as that of the first embodiment.
  • the same components as those in the first embodiment are denoted by the same reference numerals, and the description thereof is omitted as appropriate.
  • FIG. 12 (A) is a plan view showing a schematic configuration of a membrane electrode assembly provided in the fuel cell according to Embodiment 6.
  • FIG. FIG. 12B is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-1.
  • FIG. 12C is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-2.
  • FIG. 12D is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-3.
  • FIG. 13A is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-4.
  • FIG. 13B is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-5.
  • FIG. 13C is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 6-6.
  • the reinforcing layer 130 of the present embodiment includes a first band portion 232 extending in the extending direction of the interconnector 140 and a first band portion 232 extending in a direction intersecting the first band portion 232. 2 bands 234.
  • the first band 232 is disposed in a region adjacent to the interconnector 140, and the second band 234 is directed from the first band 232 toward the end of the electrolyte membrane 102 opposite to the interconnector 140. Extend.
  • the reinforcing layer 130 of the present embodiment has a shape in which the second band portion 234 protrudes from a substantially central portion of the first band portion 232 at a substantially right angle, that is, a substantially T-shape.
  • the length of one side 136 is longer than the width of the reinforcing layer 130 of the first embodiment.
  • the reinforcing layer 130 extends over the entire region in the extending direction of the interconnector 140. Thereby, the extension range of the reinforcing layer 130 in the vicinity of the interconnector 140 can be widened as compared with the first embodiment.
  • the second band portion 234 may protrude obliquely from the first band portion 232.
  • the lengths of the first band portion 232 and the second band portion 234 in the extending direction are both about 2000 ⁇ m, for example.
  • the width (the length in the direction perpendicular to the extending direction) of the first band portion 232 and the second band portion 234 is, for example, about 400 ⁇ m.
  • the reinforcing layer 130 of the present embodiment it is possible to more reliably suppress the occurrence of cracks in the vicinity of the interconnector 140 as compared with the first embodiment. As a result, a decrease in conductivity in the cathode catalyst layer 106 can be more reliably suppressed. Further, the contact area between the electrolyte membrane 102 and the cathode catalyst layer 106 can be increased as compared with the reinforcing layer 130 of the fifth embodiment, and a decrease in proton conductivity from the electrolyte membrane 102 to the cathode catalyst layer 106 is suppressed. be able to.
  • Examples of the reinforcing layer 130 of the present embodiment include the following modified examples 6-1 to 6-6.
  • the length of the first band portion 232 is shorter than that in the sixth embodiment.
  • the occurrence of cracks in the vicinity of the interconnector 140 can be suppressed more reliably than in the first embodiment, and the contact area between the electrolyte membrane 102 and the cathode catalyst layer 106 can be increased as compared with the sixth embodiment.
  • the length of the first band portion 232 of the modification 6-1 is, for example, about 1000 ⁇ m.
  • the reinforcing layer 130 of the modified example 6-2 has a plurality of second band portions 234.
  • the two second belt portions 234 are arranged so as to divide the electrolyte membrane 102 into three equal parts in the extending direction of the first belt portion 232.
  • cracks are generated in a wider range in a direction substantially perpendicular to the conductive direction in the cathode catalyst layer 106 (extending direction of the first band portion 232). Can be suppressed.
  • the width of each second belt portion 234 of Modification 6-2 is, for example, about 200 ⁇ m.
  • the total width of the two second band portions 234 is equal to the width of the second band portion 234 of the sixth embodiment and the modified example 6-1. Thereby, it is possible to avoid a decrease in the contact area between the electrolyte membrane 102 and the cathode catalyst layer 106 due to an increase in the number of the second band portions 234.
  • the reinforcing layer 130 of the modified example 6-3 has a shape obtained by combining the modified example 6-1 and the modified example 6-2, and the first belt portion 232 is formed in the fifth embodiment. It is shorter than that of the second band portion 234.
  • the occurrence of cracks in the vicinity of the interconnector 140 can be suppressed more reliably than in the first embodiment, and the electrolyte membrane 102 and the cathode catalyst layer 106 can be compared with those in the sixth embodiment and the modified example 6-2. It is possible to suppress a decrease in proton conductivity by increasing the contact area.
  • the generation of cracks can be suppressed in a wider range in the direction substantially perpendicular to the conductive direction in the cathode catalyst layer 106.
  • the reinforcing layer 130 of Modification 6-4 has a shape in which the first belt portion 232 of Modification 6-3 is divided into two.
  • a second belt portion 234 is connected to each of the two first belt portions 232.
  • the reinforcing layer 130 of the modified example 6-5 has a shape obtained by combining the sixth embodiment and the modified example 5-2, and has a first belt portion 232 and a second belt.
  • a triangular part 236 is provided instead of the part 234.
  • the triangular portion 236 has one side (bottom side) in contact with the first band portion 232, and a vertex (vertical angle) facing the one side is located at an end of the electrolyte membrane 102 opposite to the interconnector 140.
  • the reinforcing layer 130 of Modification 6-6 has a shape in which the second belt portion 234 is replaced with a triangular portion 236 in the reinforcing layer 130 of Modification 6-2. As a result, it is possible to more reliably suppress the occurrence of cracks in the vicinity of the interconnector 140 as compared with the modified example 6-2.
  • the fuel cell 10 according to the seventh embodiment is different from the first embodiment in the shape of the reinforcing layer 130 when viewed in plan.
  • this embodiment will be described.
  • the structure other than the reinforcing layer 130 of the fuel cell 10 is basically the same as that of the first embodiment.
  • the same components as those in the first embodiment are denoted by the same reference numerals, and the description thereof is omitted as appropriate.
  • FIG. 14A is a plan view showing a schematic configuration of a membrane electrode assembly provided in the fuel cell according to Embodiment 7.
  • FIG. 14B is a schematic plan view of a membrane electrode assembly in a fuel cell according to Modification 7-1.
  • the reinforcing layer 130 of the present embodiment extends in a direction intersecting the first belt portion 232 and a plurality of first belt portions 232 extending in the extending direction of the interconnector 140. It has a plurality of existing second belt portions 234 and has a substantially mesh shape.
  • the two first belt portions 232 are arranged so as to divide the electrolyte membrane 102 into three equal parts in the extending direction of the second belt portion 234, and the two second belt portions 234 separate the electrolyte membrane 102 from the first belt portion 232.
  • the part 232 is arranged so as to be divided into three equal parts in the extending direction.
  • the following modification 7-1 can be given as the reinforcing layer 130 of the present embodiment.
  • Modification 7-1 As shown in FIG. 14B, in the modified example 7-1, the length of the first belt portion 232 is shorter than that in the seventh embodiment. Thereby, compared with Embodiment 7, the contact area of the electrolyte membrane 102 and the cathode catalyst layer 106 can be enlarged, and the proton conductivity fall can be suppressed.
  • the length of the first band portion 232 of Modification 7-1 is, for example, about 1000 ⁇ m.
  • the shape of the reinforcing layer 130 is appropriately selected from any of the embodiments and modifications according to the range of the region where cracking is desired to be suppressed and the required degree of proton conductivity. Can do.
  • the reinforcing layer 130 may have a shape obtained by combining the shapes of the embodiments and the modifications.
  • the present invention can be used for fuel cells.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Fuel Cell (AREA)
  • Inert Electrodes (AREA)

Abstract

L'invention concerne une pile à combustible (10) qui comporte : un ensemble électrode à membrane (100) qui comprend une membrane électrolytique (102) qui contient un échangeur d'ions, une couche de catalyseur d'anode (104) qui est disposée sur une surface de la membrane électrolytique (102) et une couche de catalyseur de cathode (106) qui est disposée sur l'autre surface de la membrane électrolytique (102); et une couche de renfort (130) qui est enfouie dans la couche de catalyseur d'anode (104) et/ou la couche de catalyseur de cathode (106) et qui est moins apte à gonfler que la membrane électrolytique (102), tout en étant plus petite que les couches de catalyseur dans la zone projetée sur un plan qui est parallèle à la surface principale de la membrane électrolytique (102).
PCT/JP2012/000502 2011-02-28 2012-01-26 Pile à combustible WO2012117661A1 (fr)

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JP2011-043180 2011-02-28
JP2011043180A JP2014102876A (ja) 2011-02-28 2011-02-28 燃料電池

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WO2012117661A1 true WO2012117661A1 (fr) 2012-09-07

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JP2014530468A (ja) * 2011-09-23 2014-11-17 ソシエテ ビックＳｏｃｉｅｔｅ Ｂｉｃ 複合材表面に燃料電池のアレイを形成する方法
JP6005635B2 (ja) * 2011-05-20 2016-10-12 三洋電機株式会社 燃料電池

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JP6212155B2 (ja) * 2016-03-18 2017-10-11 本田技研工業株式会社 燃料電池用膜電極接合体の製造方法

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JP2003197225A (ja) * 2001-12-28 2003-07-11 Dainippon Printing Co Ltd 高分子電解質型燃料電池
JP2006252967A (ja) * 2005-03-10 2006-09-21 Nissan Motor Co Ltd 燃料電池用固体高分子電解質膜、および、これを用いた燃料電池
WO2009116630A1 (fr) * 2008-03-21 2009-09-24 旭硝子株式会社 Ensemble membrane-électrode pour pile à combustible à polymère solide, et pile à combustible à polymère solide
JP2010123511A (ja) * 2008-11-21 2010-06-03 Toyota Motor Corp 燃料電池及びその製造方法
JP2010192420A (ja) * 2009-01-23 2010-09-02 Toshiba Corp 燃料電池

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Publication number Priority date Publication date Assignee Title
JP2003197225A (ja) * 2001-12-28 2003-07-11 Dainippon Printing Co Ltd 高分子電解質型燃料電池
JP2006252967A (ja) * 2005-03-10 2006-09-21 Nissan Motor Co Ltd 燃料電池用固体高分子電解質膜、および、これを用いた燃料電池
WO2009116630A1 (fr) * 2008-03-21 2009-09-24 旭硝子株式会社 Ensemble membrane-électrode pour pile à combustible à polymère solide, et pile à combustible à polymère solide
JP2010123511A (ja) * 2008-11-21 2010-06-03 Toyota Motor Corp 燃料電池及びその製造方法
JP2010192420A (ja) * 2009-01-23 2010-09-02 Toshiba Corp 燃料電池

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP6005635B2 (ja) * 2011-05-20 2016-10-12 三洋電機株式会社 燃料電池
JP2014530468A (ja) * 2011-09-23 2014-11-17 ソシエテ ビックＳｏｃｉｅｔｅ Ｂｉｃ 複合材表面に燃料電池のアレイを形成する方法

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